Chloroform Hydrodechlorination over Palladium-Gold Catalysts: A First-Principles DFT Study

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	Chloroform Hydrodechlorination over Palladium-Gold Catalysts: A First-Principles DFT Study
	Xu, Lang 1; Yao, Xiaoqian 2; Khan, Ahmad 1; Mavrikakis, Manos 1
刊名	CHEMCATCHEM
	2016-05-09
卷号	8 期号:9 页码:1739-1746
关键词	alloys carbon chlorine density functional calculations hydrogenation
ISSN号	1867-3880
英文摘要	Hydrodechlorination is a promising method for treating toxic chlorocarbon compounds. Pd is among the most effective catalysts for chloroform hydrodechlorination, and experiments have shown that the Pd-Au alloy catalyst yields superior catalytic performance over pure Pd. Here we examine the chloroform hydrodechlorination mechanism over Pd(111) and Pd-ML/Au(111) surfaces using periodic, self-consistent density functional theory calculations (DFT, GGA-PW91) and maximum rate analysis. We suggest that the reaction occurs on both surfaces through complete dechlorination of chloroform followed by hydrogenation of CH* to methane, and that the initial dechlorination step is likely the rate-limiting step. On Pd(111), the chloroform dechlorination barrier is 0.24 eV higher than the desorption barrier, whereas on Pd-ML/Au(111), the chloroform dechlorination barrier is 0.07 eV lower than the desorption barrier, which can explain the higher hydrodechlorination activity of the Pd-Au alloy catalyst.
WOS标题词	Science & Technology ; Physical Sciences
类目[WOS]	Chemistry, Physical
研究领域[WOS]	Chemistry
关键词[WOS]	VOLATILE ORGANIC-COMPOUNDS ; TOTAL-ENERGY CALCULATIONS ; WAVE BASIS-SET ; OXIDATION ; PD ; NANOPARTICLES ; HYDROCARBONS ; HYDRODEHALOGENATION ; TRICHLOROETHYLENE ; DECHLORINATION
收录类别	SCI
语种	英语
WOS记录号	WOS:000379528500020
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/21241]
专题	过程工程研究所_多相复杂系统国家重点实验室
作者单位	1.Univ Wisconsin, Dept Chem & Biol Engn, Madison, WI 53706 USA 2.Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing Key Lab Ion Liquids Clean Proc, Beijing 100190, Peoples R China
推荐引用方式 GB/T 7714	Xu, Lang,Yao, Xiaoqian,Khan, Ahmad,et al. Chloroform Hydrodechlorination over Palladium-Gold Catalysts: A First-Principles DFT Study[J]. CHEMCATCHEM,2016,8(9):1739-1746.
APA	Xu, Lang,Yao, Xiaoqian,Khan, Ahmad,&Mavrikakis, Manos.(2016).Chloroform Hydrodechlorination over Palladium-Gold Catalysts: A First-Principles DFT Study.CHEMCATCHEM,8(9),1739-1746.
MLA	Xu, Lang,et al."Chloroform Hydrodechlorination over Palladium-Gold Catalysts: A First-Principles DFT Study".CHEMCATCHEM 8.9(2016):1739-1746.